Fluctuating hydrodynamics of multi-species reactive mixtures

Amit Kumar Bhattacharjee, Kaushik Balakrishnan, Alejandro L. Garcia, John B. Bell, Aleksandar Donev

Research output: Contribution to journalArticle

Abstract

We formulate and study computationally the fluctuating compressible Navier-Stokes equations for reactive multi-species fluid mixtures. We contrast two different expressions for the covariance of the stochastic chemical production rate in the Langevin formulation of stochastic chemistry, and compare both of them to predictions of the chemical master equation for homogeneous well-mixed systems close to and far from thermodynamic equilibrium. We develop a numerical scheme for inhomogeneous reactive flows, based on our previous methods for non-reactive mixtures [Balakrishnan, Phys. Rev. E 89, 013017 (2014)]. We study the suppression of non-equilibrium long-ranged correlations of concentration fluctuations by chemical reactions, as well as the enhancement of pattern formation by spontaneous fluctuations. Good agreement with available theory demonstrates that the formulation is robust and a useful tool in the study of fluctuations in reactive multi-species fluids. At the same time, several problems with Langevin formulations of stochastic chemistry are identified, suggesting that future work should examine combining Langevin and master equation descriptions of hydrodynamic and chemical fluctuations.

Original languageEnglish (US)
Article number224107
JournalJournal of Chemical Physics
Volume142
Issue number22
DOIs
StatePublished - Jun 14 2015

Fingerprint

Hydrodynamics
hydrodynamics
Fluids
formulations
Navier Stokes equations
Chemical reactions
Thermodynamics
chemistry
fluids
thermodynamic equilibrium
Navier-Stokes equation
chemical reactions
retarding
augmentation
predictions

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Bhattacharjee, A. K., Balakrishnan, K., Garcia, A. L., Bell, J. B., & Donev, A. (2015). Fluctuating hydrodynamics of multi-species reactive mixtures. Journal of Chemical Physics, 142(22), [224107]. https://doi.org/10.1063/1.4922308

Fluctuating hydrodynamics of multi-species reactive mixtures. / Bhattacharjee, Amit Kumar; Balakrishnan, Kaushik; Garcia, Alejandro L.; Bell, John B.; Donev, Aleksandar.

In: Journal of Chemical Physics, Vol. 142, No. 22, 224107, 14.06.2015.

Research output: Contribution to journalArticle

Bhattacharjee, AK, Balakrishnan, K, Garcia, AL, Bell, JB & Donev, A 2015, 'Fluctuating hydrodynamics of multi-species reactive mixtures', Journal of Chemical Physics, vol. 142, no. 22, 224107. https://doi.org/10.1063/1.4922308
Bhattacharjee AK, Balakrishnan K, Garcia AL, Bell JB, Donev A. Fluctuating hydrodynamics of multi-species reactive mixtures. Journal of Chemical Physics. 2015 Jun 14;142(22). 224107. https://doi.org/10.1063/1.4922308
Bhattacharjee, Amit Kumar ; Balakrishnan, Kaushik ; Garcia, Alejandro L. ; Bell, John B. ; Donev, Aleksandar. / Fluctuating hydrodynamics of multi-species reactive mixtures. In: Journal of Chemical Physics. 2015 ; Vol. 142, No. 22.
@article{9eb455b09d074d9bad597303609c14ce,
title = "Fluctuating hydrodynamics of multi-species reactive mixtures",
abstract = "We formulate and study computationally the fluctuating compressible Navier-Stokes equations for reactive multi-species fluid mixtures. We contrast two different expressions for the covariance of the stochastic chemical production rate in the Langevin formulation of stochastic chemistry, and compare both of them to predictions of the chemical master equation for homogeneous well-mixed systems close to and far from thermodynamic equilibrium. We develop a numerical scheme for inhomogeneous reactive flows, based on our previous methods for non-reactive mixtures [Balakrishnan, Phys. Rev. E 89, 013017 (2014)]. We study the suppression of non-equilibrium long-ranged correlations of concentration fluctuations by chemical reactions, as well as the enhancement of pattern formation by spontaneous fluctuations. Good agreement with available theory demonstrates that the formulation is robust and a useful tool in the study of fluctuations in reactive multi-species fluids. At the same time, several problems with Langevin formulations of stochastic chemistry are identified, suggesting that future work should examine combining Langevin and master equation descriptions of hydrodynamic and chemical fluctuations.",
author = "Bhattacharjee, {Amit Kumar} and Kaushik Balakrishnan and Garcia, {Alejandro L.} and Bell, {John B.} and Aleksandar Donev",
year = "2015",
month = "6",
day = "14",
doi = "10.1063/1.4922308",
language = "English (US)",
volume = "142",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "22",

}

TY - JOUR

T1 - Fluctuating hydrodynamics of multi-species reactive mixtures

AU - Bhattacharjee, Amit Kumar

AU - Balakrishnan, Kaushik

AU - Garcia, Alejandro L.

AU - Bell, John B.

AU - Donev, Aleksandar

PY - 2015/6/14

Y1 - 2015/6/14

N2 - We formulate and study computationally the fluctuating compressible Navier-Stokes equations for reactive multi-species fluid mixtures. We contrast two different expressions for the covariance of the stochastic chemical production rate in the Langevin formulation of stochastic chemistry, and compare both of them to predictions of the chemical master equation for homogeneous well-mixed systems close to and far from thermodynamic equilibrium. We develop a numerical scheme for inhomogeneous reactive flows, based on our previous methods for non-reactive mixtures [Balakrishnan, Phys. Rev. E 89, 013017 (2014)]. We study the suppression of non-equilibrium long-ranged correlations of concentration fluctuations by chemical reactions, as well as the enhancement of pattern formation by spontaneous fluctuations. Good agreement with available theory demonstrates that the formulation is robust and a useful tool in the study of fluctuations in reactive multi-species fluids. At the same time, several problems with Langevin formulations of stochastic chemistry are identified, suggesting that future work should examine combining Langevin and master equation descriptions of hydrodynamic and chemical fluctuations.

AB - We formulate and study computationally the fluctuating compressible Navier-Stokes equations for reactive multi-species fluid mixtures. We contrast two different expressions for the covariance of the stochastic chemical production rate in the Langevin formulation of stochastic chemistry, and compare both of them to predictions of the chemical master equation for homogeneous well-mixed systems close to and far from thermodynamic equilibrium. We develop a numerical scheme for inhomogeneous reactive flows, based on our previous methods for non-reactive mixtures [Balakrishnan, Phys. Rev. E 89, 013017 (2014)]. We study the suppression of non-equilibrium long-ranged correlations of concentration fluctuations by chemical reactions, as well as the enhancement of pattern formation by spontaneous fluctuations. Good agreement with available theory demonstrates that the formulation is robust and a useful tool in the study of fluctuations in reactive multi-species fluids. At the same time, several problems with Langevin formulations of stochastic chemistry are identified, suggesting that future work should examine combining Langevin and master equation descriptions of hydrodynamic and chemical fluctuations.

UR - http://www.scopus.com/inward/record.url?scp=84934971275&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84934971275&partnerID=8YFLogxK

U2 - 10.1063/1.4922308

DO - 10.1063/1.4922308

M3 - Article

VL - 142

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 22

M1 - 224107

ER -